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Silk fibroin (SF), the primary protein in silkworm silk, has emerged as a promising organic nonlinear optical material due to its unique combination of optical transparency, biocompatibility, and environmental sustainability. In this study, we investigate the nonlinear optical properties of SF thin films using the z-scan technique with femtosecond laser pulses (35 fs, 800 nm, 1 kHz). Our results reveal a strong self-defocusing effect (negative nonlinear refractive index) and significant multiphoton absorption, demonstrating SF’s tunable nonlinear response. Additionally, optical transmittance measurements confirm SF’s partial transparency in the deep UV region, enhancing its potential for second-harmonic generation (SHG) and efficient light frequency conversion. These findings address a key knowledge gap in nonlinear optics, positioning SF as a versatile biopolymer for advanced photonic applications.

We present the results of an experimental study of multiphoton ionization in fused silica, using a linearly polarized femtosecond Satsuma fiber laser with an active medium based on Yb+3 ions, at 515 -nm and 1030 -nm wavelengths. The radiation transmission in the fused silica was measured as a function of the laser intensity and wavelength and the data were analyzed using a theoretical model based on the Keldysh theory. We determined the multiphoton absorption cross-sections in the fused silica in the case of four- and eight-photon ionization and analyzed the contribution of avalanche ionization. The obtained results provide insight into the fundamental processes involved in multiphoton ionization and have implications for its applications, such as laser micromachining and material processing.

Expressions for the spectral and temperature dependences of the partial coefficients of interband multiphoton absorption of light are determined, which differ from each other by the types of virtual optical transitions, depending on the degree of polarization of light. A quantitative analysis of the coefficient of multiphoton interband linear-circular dichroism is carried out. A quantitative analysis of the spectral dependence of two and three-photon interband light absorption in the InSb semiconductor is carried out, the quantitative calculation of which is based on perturbation theory in the Kane approximation, where the energy spectrum of current carriers is assumed to be spherically symmetric.

Temporal focusing, with its ability to focus light in time, enables scanless illumination of large surface areas at the sample with micrometer axial confinement and robust propagation through scattering tissue. In conventional two-photon microscopy, widely used for the investigation of intact tissue in live animals, images are formed by point scanning of a spatially focused pulsed laser beam, resulting in limited temporal resolution of the excitation. Replacing point scanning with temporally focused widefield illumination removes this limitation and represents an important milestone in two-photon microscopy. Temporal focusing uses a diffusive or dispersive optical element placed in a plane conjugate to the objective focal plane to generate position-dependent temporal pulse broadening that enables axially confined multiphoton absorption, without the need for tight spatial focusing. Many techniques have benefitted from temporal focusing, including scanless imaging, super-resolution imaging, photolithography, uncaging of caged neurotransmitters and control of neuronal activity via optogenetics. This Review discusses temporal focusing microscopy and its applications in neuroscience for imaging and optogenetic activation.

All-inorganic CsPbX 3 (X = Cl, Br, and I) perovskite quantum dots (PeQDs) have shown great promise in optoelectronics and photovoltaics owing to their outstanding linear optical properties; however, nonlinear upconversion is limited by the small cross-section of multiphoton absorption, necessitating high power density excitation. Herein, we report a convenient and versatile strategy to fine tuning the upconversion luminescence in CsPbX 3 PeQDs through sensitization by lanthanide-doped nanoparticles. Full-color emission with wavelengths beyond the availability of lanthanides is achieved through tailoring of the PeQDs bandgap, in parallel with the inherent high conversion efficiency of energy transfer upconversion under low power density excitation. Importantly, the luminescent lifetimes of the excitons can be enormously lengthened from the intrinsic nanosecond scale to milliseconds depending on the lifetimes of lanthanide ions. These findings provide a general approach to stimulate photon upconversion in PeQDs, thereby opening up a new avenue for exploring novel and versatile applications of PeQDs. Optimizing luminescence from quantum dots benefits various optoelectronic and photovoltaic applications. Here the authors drive high-efficiency, tunable upconversion luminescence in perovskite quantum dots by energy transfer from lanthanide-doped nanoparticles excited by near-infrared light, to produce full-color emission with low driving power.

It’s critically important to construct arbitrary inorganic features with high resolution. As an inorganic photoresist, hydrogen silsesquioxane (HSQ) has been patterned by irradiation sources with short wavelength, such as EUV and electron beam. However, the fabrication of three- dimensional nanoscale HSQ features utilizing infrared light sources is still challenging. Here, we demonstrate femtosecond laser direct writing (FsLDW) of HSQ through multi-photon absorption process. 26 nm feature size is achieved by using 780 nm fs laser, indicating super-diffraction limit photolithography of λ/30 for HSQ. HSQ microstructures by FsLDW possess nanoscale resolution, smooth surface, and thermal stability up to 600 °C. Furthermore, we perform FsLDW of HSQ to construct structural colour and Fresnel lens with desirable optical properties, thermal and chemical resistance. This study demonstrates that inorganic features can be flexibly achieved by FsLDW of HSQ, which would be prospective for fabricating micro-nano devices requiring nanoscale resolution, thermal and chemical resistance. Stereolithography has progressed over the years but resolution and feature size is still limited by the properties of materials and resins. Here, the authors demonstrate femtosecond laser direct writing of a hydrogen silsesquioxane photoresist using a 780 nm femtosecond laser demonstrating feature sizes of 26 nm.

Imitating the natural photosynthesis to synthesize hydrocarbon fuels represents a viable strategy for solar-to-chemical energy conversion, where utilizing low-energy photons, especially near-infrared photons, has been the ultimate yet challenging aim to further improving conversion efficiency. Plasmonic metals have proven their ability in absorbing low-energy photons, however, it remains an obstacle in effectively coupling this energy into reactant molecules. Here we report the broadband plasmon-induced CO 2 reduction reaction with water, which achieves a CH 4 production rate of 0.55 mmol g −1 h −1 with 100% selectivity to hydrocarbon products under 400 mW cm −2 full-spectrum light illumination and an apparent quantum efficiency of 0.38% at 800 nm illumination. We find that the enhanced local electric field plays an irreplaceable role in efficient multiphoton absorption and selective energy transfer for such an excellent light-driven catalytic performance. This work paves the way to the technique for low-energy photon utilization. Changes in Polycomb repression during interphase transition modulate the ability of pluripotent cells to enter cell differentiation.

Multiphoton upconversion is a process where two or more photons are absorbed simultaneously to excite an electron to an excited state and, subsequently, the relaxation of electron gives rise to the emission of a photon with frequency greater than those of the absorbed photons. Materials possessing such property attracted attention due to applications in biological imaging, photodynamic therapy, three-dimensional optical data storage, frequency-upconverted lasing and optical power limiting. Here we report four-photon upconversion in metal–organic frameworks containing the ligand, trans , trans -9,10-bis(4-pyridylethenyl)anthracene. The ligand has a symmetrical acceptor–π–donor–π–acceptor structure and a singlet biradical electronic ground state, which boosted its multiphoton absorption cross-sections. We demonstrate that the upconversion efficiency can be enhanced by Förster resonance energy transfer within host–guest metal–organic frameworks consisting of encapsulated high quantum yielding guest molecules. Using these strategies, metal–organic framework materials, which can exhibit frequency-upconverted photoluminescence excited by simultaneous multiphoton absorption, can be rationally designed and synthesized. Metal–organic frameworks (MOFs) combining the properties of the metal ions and organic ligands are been proposed for many applications. Here Quah et al . demonstrate multiphoton excitation fluorescence in MOF materials enhanced by high quantum yielding guest molecules and Förster resonance energy transfer.

To combine the advantages of ultrafast femtosecond nano-optics with an on-chip communication scheme, optical signals with a frequency of several hundreds of THz need to be down-converted to coherent electronic signals propagating on-chip. So far, this has not been achieved because of the overall slow response time of nanoscale electronic circuits. Here, we demonstrate that 14 fs optical pulses in the near-infrared can drive electronic on-chip circuits with a prospective bandwidth up to 10 THz. The corresponding electronic pulses propagate in macroscopic striplines on a millimeter scale. We exploit femtosecond photoswitches based on asymmetric, nanoscale metal junctions to drive the pulses. The non-linear ultrafast response is based on a plasmonically enhanced, multiphoton absorption resulting in a field emission of ballistic hot electrons propagating across the nanoscale junctions. Our results pave the way towards femtosecond electronics integrated in wafer-scale THz circuits. For future ultrafast opto-electronic circuits, optical signals must be interfaced with coherent electronic signals. The authors develop asymmetric plasmonic nanojunctions that convert fs light pulses to THz electronic transients that can propagate on-chip for up to a mm, enabling such an interface.

Organic nonlinear optical materials have potential in applications such as lightings and bioimaging, but tend to have low photoluminescent quantum yields and are prone to lose the nonlinear optical activity. Herein, we demonstrate to weave large-area, flexible organic nonlinear optical membranes composed of 4-N,N-dimethylamino-4ʹ-Nʹ-methyl-stilbazolium tosylate@cyclodextrin host-guest supramolecular complex. These membranes exhibited a record high photoluminescence quantum yield of 73.5%, and could continuously emit orange luminescence even being heated at 300 °C, thus enabling the fabrication of thermotolerant light-emitting diodes. The nonlinear optical property of these membranes can be well-preserved even in polar environment. The supramolecular assemblies with multiphoton absorption characteristics were used for in vivo real-time imaging of Escherichia coli at 1000 nm excitation. These findings demonstrate to achieve scalable fabrication of organic nonlinear optical materials with high photoluminescence quantum yields, and good stability against thermal stress and polar environment for high-performance, durable optoelectronic devices and humanized multiphoton bio-probes. Organic nonlinear optical materials have potential in applications such as bioimaging, but tend to have low photoluminescent quantum yields and are prone to aggregation-caused quenching. Here, the authors report a host-guest approach for improving the luminescent properties of these materials.